Dual stimuli-responsive multicompartment micelles from triblock terpolymers with tunable hydrophilicity

Betthausen, Eva; Drechsler, Markus; Förtsch, Melanie; Schacher, Felix H.; Müller, Axel H. E.

doi:10.1039/c1sm05822c

Cited by 77 publications

(130 citation statements)

References 39 publications

Supporting

Mentioning

124

Contrasting

Order By: Relevance

“…While polymeric coronas often are not visible in cryo-TEM due to their hydrated nature; the direct visualization of micelle coronas (including PNIPAM) has been reported previously. 36, 38, 56, 60-62 As seen in Figure 2, cryo-TEM further supported that the amphiphilic homopolymer formed spherical micelles in aqueous solutions. Moreover, assuming mass-thickness contrast dominates (i.e.…”

Section: Resultssupporting

confidence: 52%

Structural Characterization of Amphiphilic Homopolymer Micelles Using Light Scattering, SANS, and Cryo-TEM

et al. 2013

View full text Add to dashboard Cite

We report the aqueous solution self-assembly of a series of poly(N-isopropylacrylamide) (PNIPAM) polymers end-functionalized with a hydrophobic sulfur-carbon-sulfur (SCS) pincer ligand. Although the hydrophobic ligand accounted for <5 wt% of the overall homopolymer mass, the polymers self-assembled into well-defined spherical micelles in aqueous solution, and these micelles are potential precursors to solution-assembled nanoreactors for small molecule catalysis applications. The micelle structural details were investigated using light scattering, cryogenic transmission electron microscopy (cryo-TEM), and small angle neutron scattering (SANS). Radial density profiles extracted from the cryo-TEM micrographs suggested that the PNIPAM chains formed a diffuse corona with a radially decreasing corona density profile and provided valuable a priori information about the micelle structure for SANS data modeling. SANS analysis indicated a similar profile in which the corona surrounded a small hydrophobic core containing the pincer ligand. The similarity between the SANS and cryo-TEM results demonstrated that detailed information about the micelle density profile can be obtained directly from cryo-TEM and highlighted the complementary use of scattering and cryo-TEM in the structural characterization of solution-assemblies, such as the SCS pincer-functionalized homopolymers described here.

show abstract

Section: Resultssupporting

confidence: 52%

Structural Characterization of Amphiphilic Homopolymer Micelles Using Light Scattering, SANS, and Cryo-TEM

et al. 2013

View full text Add to dashboard Cite

show abstract

“…Comparable chain rearrangements have been shown for BMAAD triblock terpolymer micelles of 120-200 nm size at different pH values. 34 However, such subtle morphological changes are difficult if not impossible to verify using electron microscopy for such small nanostructures (sub 30 nm). Furthermore, the two situations depicted in Figure 4 represent the extreme morphological states, and the true situation during encapsulation might be located in between.…”

Section: V19-05048 As Surrogate Cargomentioning

confidence: 99%

Cargo–carrier interactions significantly contribute to micellar conformation and biodistribution

et al. 2017

View full text Add to dashboard Cite

Strategies to deliver drugs using nanocarriers, which are passively or actively targeted to their alleged site of action might favorably affect benefit-risk profiles of novel therapeutics. Here we tested the hypothesis whether the physico-chemical properties of the cargo as well as the actual conditions during encapsulation interfere during formulation of nanoparticular cargo-carrier systems. On the basis of previous work, a versatile class of nanocarriers is polyether-based ABC triblock terpolymer micelles with diameters below 50 nm. Their tunable chemistry and size allows to systematically vary important parameters. We demonstrate in vivo differences in pharmacokinetics and biodistribution not only dependent on micellar net charge but also on the properties of encapsulated (model) drugs and their localization within the micelles. On the basis of in vitro and in vivo evidence we propose that depending on drug cargo and encapsulation conditions micelles with homogeneous or heterogeneous corona structure are formed, contributing to an altered pharmacokinetic profile as differences in cargo location occur. Thus, these interactions have to be considered when a carrier system is selected to achieve optimal delivery to a given tissue.

show abstract

“…Since styrene is similar in reactivity to 1,3-butadiene, another sequentially different triblock terpolymer of PB-b-PS-b-P t BMA may be synthesized by changing the addition order of styrene and 1,3-butadiene. Furthermore, the following triblock terpolymers, belonging to the same category, were also synthesized by means of the same sequential polymerization technique with a careful monomer addition order: [41], and PS-b-Poly(2-trimethhylsilyloxyethyl methacrylate)-b-PMMA [42].…”

Section: Synthesis Of Block Polymers By Sequential Polymerizationmentioning

confidence: 99%

Precise Synthesis of Block Polymers Composed of Three or More Blocks by Specially Designed Linking Methodologies in Conjunction with Living Anionic Polymerization System

et al. 2013

View full text Add to dashboard Cite

This article reviews the successful development of two specially designed linking methodologies in conjunction with a living anionic polymerization system for the synthesis of novel multiblock polymers, composed of three or more blocks, difficult to be synthesized by sequential polymerization. The first methodology with the use of a new heterofunctional linking agent, 2-(4-chloromethylphenyl)ethyldimethylchlorosilane (1), was developed for the synthesis of multiblock polymers containing poly(dimethylsiloxane) (PDMS) blocks. This methodology is based on the selective reaction of the chain-end silanolate anion of living PDMS, with the silyl chloride function of 1, and subsequent linking reaction of the resulting ω-chain-end-benzyl chloride-functionalized polymer with either a living anionic polymer or living anionic block copolymer. With this methodology, various multiblock polymers containing PDMS blocks, up to the pentablock quintopolymer, were successfully synthesized. The second methodology using an α-phenylacrylate (PA) reaction site was developed for the synthesis of multiblock polymers composed of all-vinyl polymer blocks. In this methodology, an α-chain-end-PA-functionalized polymer or block copolymer, via the living anionic polymerization, was first prepared and, then, reacted with appropriate living anionic polymer or block copolymer to link the two polymer chains. As OPEN ACCESSPolymers 2013, 5 1013 a result, ACB (BCA), BAC (CAB), (AB) n , (AC) n , ABA, ACA, BCB, and ABCA multiblock polymers, where A, B, and C were polystyrene, poly(2-vinylpyridine), and poly(methyl methacrylate) segments, could be successfully synthesized. The synthesis of triblock copolymers, BAB, CAC, and CBC, having molecular asymmetry in both side blocks, was also achieved. Furthermore, the use of living anionic polymers, derived from many other monomers, categorized as either of styrene, 2-vinylpyridine, or methyl methacrylate in monomer reactivity, in the linking methodology enabled the number of synthetically possible block polymers to be greatly increased. Once again, all of the block polymers synthesized by these methodologies are new and cannot be synthesized at all by sequential polymerization. They were well-defined in block architecture and precisely controlled in block segment.

show abstract

Dual stimuli-responsive multicompartment micelles from triblock terpolymers with tunable hydrophilicity

Cited by 77 publications

References 39 publications

Structural Characterization of Amphiphilic Homopolymer Micelles Using Light Scattering, SANS, and Cryo-TEM

Structural Characterization of Amphiphilic Homopolymer Micelles Using Light Scattering, SANS, and Cryo-TEM

Cargo–carrier interactions significantly contribute to micellar conformation and biodistribution

Precise Synthesis of Block Polymers Composed of Three or More Blocks by Specially Designed Linking Methodologies in Conjunction with Living Anionic Polymerization System

Contact Info

Product

Resources

About